Sophie Ayrault

Radiocesium transfer from hillslopes to the Pacific Ocean after the Fukushima Nuclear Power Plant accident: A review

The devastating tsunami triggered by the Great East Japan Earthquake on March 11, 2011 inundated the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) resulting in a loss of cooling and a series of explosions releasing the largest quantity of radioactive material into the atmosphere since the Chernobyl nuclear accident. Although 80% of the radionuclides from this accidental release were transported over the Pacific Ocean, 20% were deposited over Japanese coastal catchments that are subject to frequent typhoons. Among the radioisotopes released during the FDNPP accident, radiocesium ((134)Cs and (137)Cs) is considered the most serious current and future health risk for the local population. The goal of this review is to synthesize research relevant to the transfer of FDNPP derived radiocesium from hillslopes to the Pacific Ocean. After radiocesium fallout deposition on vegetation and soils, the contamination may remain stored in forest canopies, in vegetative litter on the ground, or in the soil. Once radiocesium contacts soil, it is quickly and almost irreversibly bound to fine soil particles. The kinetic energy of raindrops instigates the displacement of soil particles, and their bound radiocesium, which may be mobilized and transported with overland flow. Soil erosion is one of the main processes transferring particle-bound radiocesium from hillslopes through rivers and streams, and ultimately to the Pacific Ocean. Accordingly this review will summarize results regarding the fundamental processes and dynamics that govern radiocesium transfer from hillslopes to the Pacific Ocean published in the literature within the first four years after the FDNPP accident. The majority of radiocesium is reported to be transported in the particulate fraction, attached to fine particles. The contribution of the dissolved fraction to radiocesium migration is only relevant in base flows and is hypothesized to decline over time. Owing to the hydro-meteorological context of the Fukushima region, the most significant transfer of particulate-bound radiocesium occurs during major rainfall and runoff events (e.g. typhoons and spring snowmelt). There may be radiocesium storage within catchments in forests, floodplains and even within hillslopes that may be remobilized and contaminate downstream areas, even areas that did not receive fallout or may have been decontaminated. Overall this review demonstrates that characterizing the different mechanisms and factors driving radiocesium transfer is important. In particular, the review determined that quantifying the remaining catchment radiocesium inventory allows for a relative comparison of radiocesium transfer research from hillslope to catchment scales. Further, owing to the variety of mechanisms and factors, a transdisciplinary approach is required involving geomorphologists, hydrologists, soil and forestry scientists, and mathematical modellers to comprehensively quantify radiocesium transfers and dynamics. Characterizing radiocesium transfers from hillslopes to the Pacific Ocean is necessary for ongoing decontamination and management interventions with the objective of reducing the gamma radiation exposure to the local population.

Tracing sediment sources in a tropical highland catchment of central Mexico by using conventional and alternative fingerprinting methods

Land degradation is intense in tropical regions where it causes for instance a decline in soil fertility and reservoir siltation. Two fingerprinting approaches (i.e. the conventional approach based on radionuclide and geochemical concentrations and the alternative diffuse reflectance infrared Fourier transform spectroscopy method) were conducted independently to outline the sources delivering sediment to the river network draining into the Cointzio reservoir, in Mexican tropical highlands. This study was conducted between May and October in 2009 in subcatchments representative of the different environments supplying sediment to the river network. Overall, Cointzio catchment is characterized by very altered soils and the dominance of Andisols and Acrisols. Both fingerprinting methods provided very similar results regarding the origin of sediment in Huertitas subcatchment (dominated by Acrisols) where the bulk of sediment was supplied by gullies. In contrast, in La Cortina subcatchment dominated by Andisols, the bulk of sediment was supplied by cropland. Sediment originating from Potrerillos subcatchment characterized by a mix of Acrisols and Andisols was supplied in variable proportions by both gullies and rangeland/cropland. In this latter subcatchment, results provided by both fingerprinting methods were very variable. Our results outline the need to take the organic carbon content of soils into account and the difficulty to use geochemical properties to fingerprint sediment in very altered volcanic catchments. However, combining our fingerprinting results with sediment export data provided a way of prioritizing the implementation of erosion control measures to mitigate sediment supply to the Cointzio reservoir supplying drinking water to Morelia city. Copyright

Evolution of radioactive dose rates in fresh sediment deposits along coastal rivers draining Fukushima contamination plume

Measurement of radioactive dose rates in fine sediment that has recently deposited on channel bed-sand provides a solution to address the lack of continuous river monitoring in Fukushima Prefecture after Fukushima Dai-ichi nuclear power plant (FDNPP) accident. We show that coastal rivers of Eastern Fukushima Prefecture were rapidly supplied with sediment contaminated by radionuclides originating from inland mountain ranges, and that this contaminated material was partly exported by typhoons to the coastal plains as soon as by November 2011. This export was amplified during snowmelt and typhoons in 2012. In 2013, contamination levels measured in sediment found in the upper parts of the catchments were almost systematically lower than the ones measured in nearby soils, whereas their contamination was higher in the coastal plains. We thereby suggest that storage of contaminated sediment in reservoirs and in coastal sections of the river channels now represents the most crucial issue.

Tracing sediment sources in a tropical highland catchment of central Mexico by using conventional and alternative fingerprinting methodsTracing sediment sources in a tropical

Land degradation is intense in tropical regions where it causes for instance a decline in soil fertility and reservoir siltation. Two fingerprinting approaches (i.e. the conventional approach based on radionuclide and geochemical concentrations and the alternative diffuse reflectance infrared Fourier transform spectroscopy method) were conducted independently to outline the sources delivering sediment to the river network draining into the Cointzio reservoir, in Mexican tropical highlands. This study was conducted between May and October in 2009 in subcatchments representative of the different environments supplying sediment to the river network. Overall, Cointzio catchment is characterized by very altered soils and the dominance of Andisols and Acrisols. Both fingerprinting methods provided very similar results regarding the origin of sediment in Huertitas subcatchment (dominated by Acrisols) where the bulk of sediment was supplied by gullies. In contrast, in La Cortina subcatchment dominated by Andisols, the bulk of sediment was supplied by cropland. Sediment originating from Potrerillos subcatchment characterized by a mix of Acrisols and Andisols was supplied in variable proportions by both gullies and rangeland/cropland. In this latter subcatchment, results provided by both fingerprinting methods were very variable. Our results outline the need to take the organic carbon content of soils into account and the difficulty to use geochemical properties to fingerprint sediment in very altered volcanic catchments. However, combining our fingerprinting results with sediment export data provided a way of prioritizing the implementation of erosion control measures to mitigate sediment supply to the Cointzio reservoir supplying drinking water to Morelia city. Copyright

Interspecies calibration in mosses at regional scale—heavy metal and trace elements results from Ile-de-France

Abstract This is the first attempt in France to determine the interspecies comparisons of heavy metal and trace elemental concentrations by analysing terrestrial moss species. This study was conducted mainly around Paris, in the Ile-de-France area which is known as one of the regions in France with highly industrialized and urban locations. The mosses were collected within the framework of a European-scale campaign on background pollution carried out in France (1995–1996). A large diversity of species are usually sampled in large-scale surveys which poses problems for interspecies calibration. As regards this intercomparison study, paired samples of Hypnum cupressiforme, Pleurozium schreberi and Scleropodium purum were collected at a total of 20 sampling points. The study was on three species because large numbers of these moss species were sampled in France during the 1996 biomonitoring campaign. The samples were analysed for 36 elements using both analytical methods by instrumental neutron activation analysis (INAA) and inductively coupled plasma-mass spectrometry (ICP-MS). Element concentrations in moss species were compared using correlation by linear regression. The study showed that the pair H. cupressiforme and P. schreberi and the pair H. cupressiforme and S. purum can be used interchangeably as biomonitors in the Ile-de-France area for Al, As, Co, Cs, Fe, La, Mn, Rb, Sc, Sm, V and for Cl, Mn, Pb, Rb, Sb, Zn, respectively. In many cases interspecies calibration is not possible potentially due to saturation effect in one species, especially H. cupressiforme. Finally, the use of reliable calibration factors is recommended in Ile-de-France data sets for caesium and rubidium (Ps–Hc) or antimony, lead and rubidium (Sp–Hc) because the correlation is significant at a 99% confidence interval at least and the mean ratio calculated between both moss species differs significantly from 1.0.

Renewed soil erosion and remobilisation of radioactive sediment in Fukushima coastal rivers after the 2013 typhoons

Summer typhoons and spring snowmelt led to the riverine spread of continental Fukushima fallout to the coastal plains of Northeastern Japan and the Pacific Ocean. Four fieldwork campaigns based on measurement of radioactive dose rates in fine riverine sediment that has recently deposited on channel bed-sand were conducted between November 2011 and May 2013 to document the spread of fallout by rivers. After a progressive decrease in the fresh riverine sediment doses rates between 2011 and early spring in 2013, a fifth campaign conducted in November 2013 showed that they started to increase again after the occurrence of violent typhoons. We show that this increase in dose rates was mostly due to remobilization of contaminated material that was temporarily stored in river channels or, more importantly, in dam reservoirs of the region during the typhoons. In addition, supply of particles from freshly eroded soils in autumn 2013 was the most important in areas where decontamination works are under progress. Our results underline the need to monitor the impact of decontamination works and dam releases in the region, as they may provide a continuous source of radioactive contamination to the coastal plains and the Pacific Ocean during the coming years.

Spatio-temporal variability of solid, total dissolved and labile metal: passive vs. discrete sampling evaluation in river metal monitoring

In order to obtain representative dissolved and solid samples from the aquatic environment, a spectrum of sampling methods are available, each one with different advantages and drawbacks. This article evaluates the use of discrete sampling and time-integrated sampling in illustrating medium-term spatial and temporal variation. Discrete concentration index (CI) calculated as the ratio between dissolved and solid metal concentrations in grab samples are compared with time-integrated concentration index (CI) calculated from suspended particulate matter (SPM) collected in sediment traps and labile metals measured by the diffusive gel in thin films (DGT) method, collected once a month during one year at the Seine River, upstream and downstream of the Greater Paris Region. Discrete CI at Bougival was found to be significantly higher than at Triel for Co, Cu, Mn, Ni and Zn, while discrete metal partitioning at Marnay was found to be similar to Bougival and Triel. However, when using time-integrated CI, not only was Bougival CI significantly higher than Triel CI, CI at Marnay was also found to be significantly higher than CI at Triel which was not observed for discrete CI values. Since values are time-averaged, dramatic fluctuations were smoothed out and significant medium-term trends were enhanced. As a result, time-integrated concentration index (CI) was able to better illustrate urbanization impact between sites when compared to discrete CI. The impact of significant seasonal phenomenon such as winter flood, low flow and redox cycles was also, to a certain extent, visible in time-integrated CI values at the upstream site. The use of time-integrated concentration index may be useful for medium- to long-term metal studies in the aquatic environment.

X-ray absorption fine structure evidence for amorphous zinc sulfide as a major zinc species in suspended matter from the Seine River downstream of Paris, Ile-de-France, France.

Zinc is one of the most widespread trace metals (TMs) in Earth surface environments and is the most concentrated TM in the downstream section of the Seine River (France) due to significant anthropogenic input from the Paris conurbation. In order to better identify the sources and cycling processes of Zn in this River basin, we investigated seasonal and spatial variations of Zn speciation in suspended particulate matter (SPM) in the oxic water column of the Seine River from upstream to downstream of Paris using synchrotron-based extend X-ray absorption fine structure (EXAFS) spectroscopy at the Zn K-edge. First-neighbor contributions to the EXAFS were analyzed in SPM samples, dried and stored under a dry nitrogen atmosphere or under an ambient oxygenated atmosphere. We found a sulfur first coordination environment around Zn (in the form of amorphous zinc sulfide) in the raw SPM samples stored under dry nitrogen vs an oxygen first coordination environment around Zn in the samples stored in an oxygenated atmosphere. These findings are supported by scanning electron microscopy and energy dispersive X-ray spectrometry observations. Linear combination fitting of the EXAFS data for SPM samples, using a large set of EXAFS spectra of Zn model compounds, indicates dramatic changes in the Zn speciation from upstream to downstream of Paris, with amorphous ZnS particles becoming dominant dowstream. In contrast, Zn species associated with calcite (either adsorbed or incorporated in the structure) are dominant upstream. Other Zn species representing about half of the Zn pool in the SPM consist of Zn-sorbed on iron oxyhydroxides (ferrihydrite and goethite) and, to a lesser extent, Zn-Al layered double hydroxides, Zn incorporated in dioctahedral layers of clay minerals and Zn sorbed to amorphous silica. Our results highlight the importance of preserving the oxidation state in TM speciation studies when sampling suspended matter, even in an oxic water column.

Urbanization impact on metals mobility in riverine suspended sediment: Role of metal oxides

Spatial and temporal fractionation of trace metals and major elements in suspended particulate matter in the Seine River was investigated to study the impact of the increasing urbanization in the Greater Paris Region. Suspended sediments in the Seine River were collected between December 2008 to August 2009 upstream and downstream of Paris. They were subjected to total digestion and sequential extraction procedure certified by the Bureau Communautaire de Référence and trace metals along with major elements were analyzed with inductively coupled plasma mass spectroscopy. Metal enrichment factors increased up to eight folds after the Seine River downstream of the Greater Paris Region showing a significant contribution of urbanization. Enrichment of copper, lead and zinc downstream of Paris are followed by the increase of their reducible fraction of at least 10% implicating an increase in metals associated with iron oxides. The exchangeable fraction, which includes the carbonate-associated metals, is only significant for cadmium, nickel and zinc (more than 2 %) while the oxidisable fraction accounts for less than 20 % for the anthropogenic metals downstream except for copper. The metals can be divided to (a) “reducible” group including cadmium, lead, and zinc, associated with more than 60 % of the total Bureau Communautaire de Référence extractable metals to the reducible fraction containing mostly iron oxide phases for the downstream sites. (b) A “distributed” group including chromium, copper, and nickel that are associated to at least 3 different phase-groups: (1) oxides, (2) organic matter and sulphides and (3) mineral phases.

Bioavailability of particulate metal to zebra mussels: Biodynamic modelling shows that assimilation efficiencies are site-specific

This study investigates the ability of the biodynamic model to predict the trophic bioaccumulation of cadmium (Cd), chromium (Cr), copper (Cu), nickel (Ni) and zinc (Zn) in a freshwater bivalve. Zebra mussels were transplanted to three sites along the Seine River (France) and collected monthly for 11 months. Measurements of the metal body burdens in mussels were compared with the predictions from the biodynamic model. The exchangeable fraction of metal particles did not account for the bioavailability of particulate metals, since it did not capture the differences between sites. The assimilation efficiency (AE) parameter is necessary to take into account biotic factors influencing particulate metal bioavailability. The biodynamic model, applied with AEs from the literature, overestimated the measured concentrations in zebra mussels, the extent of overestimation being site-specific. Therefore, an original methodology was proposed for in situ AE measurements for each site and metal.